Cellulose-based triboelectric nanogenerators (TENGs) are increasingly studied as potential candidates for advancing sustainable wearable electronics due to their biodegradability, self-powering capability, and high sensitivity. However, the near-electroneutrality of cellulose and its lack of efficient charge storage sites result in rapid charge dissipation. This study’s synergistic approach of constructing deep traps and built-in electric fields effectively promotes charge trapping. This approach achieved nearly 2 orders of magnitude improvement in the deep-trap density of the modified cellulose and a 74% reduction in the charge dissipation rate, compared with cellulose, yielding a charge density as high as 332 μC/m2, comparable to the output produced by the ion injection. The integrated TENG demonstrates reliable and high-sensitivity signal transmission as a wearable electronic device. This study presents a simple and scalable strategy for fabricating high-performance cellulose-based TENGs, underscoring the significant potential of cellulose in sustainable self-powered wearable electronics.